4.6 Article

Experimental and Theoretical Studies on Water-Added Thermal Processing of Model Biosyngas for Improving Hydrogen Production and Restraining Soot Formation

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AMER CHEMICAL SOC
DOI: 10.1021/acs.iecr.2c01680

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  1. Chevron
  2. Norwegian Research Council
  3. Gas Technology Centre at NTNU/SINTEF
  4. Statoil
  5. Vista
  6. NTNU
  7. SINTEF

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The upgrading of biosyngas to convert methane into syngas is a crucial step for hydrogen production from biomass. This study investigates the thermal treatment of a model biosyngas and examines the effects of various variables on the reaction. The proposed reaction mechanism involves dry reforming of methane, reverse water-gas shift reactions, and methane pyrolysis. Additionally, the study reveals the presence of SiO2 species as a support for carbon formation, resulting from the chemical reaction between the reactor wall material and the reactants.
The upgrading of biosyngas to convert methane into syngas is a necessary step for hydrogen production from biomass. However, this process is highly energy-demanding. In this study, a model biosyngas containing H-2, CH4, CO, and CO2 were thermally treated between 1200 and 1500 degrees C. The gas mixture, comprised of H-2 (33 Vol %), CH4 (12 Vol %), CO (28 vol %), CO2 (25 vol %), and He (2 vol %), was diluted with argon and the effect of reaction temperature (1200-1500 degrees C), water addition (0-44.3 mol %), and residence time (23, 46, and 76 mu s in corresponding to flow rates of 1500, 2500, and 5000 inLimin at normal temperature and pressure, respectively) were studied. A possible reaction scheme for the upgrading of the model gas is proposed based on the kinetic simulation with CHEMKIN. The main reaction pathways involve dry reforming of methane and reverse water-gas shift (WGS) reactions. The kinetic simulation explained the finding that CO production was negatively influenced by the water content via the WGS reaction. The main side reaction is the methane pyrolysis reaction which causes the formation of carbon. The carbon formed in the reforming was characterized by SEM and Raman spectroscopy. SiO2 needle-like microdomains are observed at the top of the reactor heating zone, while the central part of the heating zone was covered by carbon with a disordered, amorphous, low-density soot structure. It is proposed that the SiO2 species formed by the chemical reaction between the reactor wall material and the reactants act as a support to anchor the carbon formed.

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